Proton beam writing of microstructures at the ion nanoprobe LIPSION

Proton beam writing (PBW) is a direct writing technique which allows the creation of three-dimensional structures with a high aspect ratio in the micrometer and nanometer range in photoresist materials without the use of templates. At the high-energy ion nanoprobe LIPSION of the University of Leipzig this technique was established recently. In this article the latest results concerning this topic are presented. PBW was successfully performed with the positive resist polymethyl methacrylate (PMMA) which is now used at LIPSION in addition to the negative resist SU-8. With the new data acquisition system MICRODAS being commissioned, a new scan program was developed and tested which is dedicated to the creation of arbitrarily shaped structures. Squares with dimensions down to 1.2 μm were created in SU-8 at LIPSION. Furthermore, Ni grids were produced by electroplating, using templates written in PMMA resist. In addition, first structures for studying the growing behavior of Bragg reflectors and the optical characterisation of ZnO nanowhiskers were produced by PBW.     

Proton beam writing of microstructures in Agar gel for patterned cell growth

A rather useful prerequisite for many biological and biophysical studies, e.g., for cell-cell communication or neuronal networks, is confined cell growth on micro-structured surfaces. Solidified Agar layers have smooth surfaces which are electrically neutral and thus inhibit receptor binding and cell adhesion. For the first time, Agar microstructures have been manufactured using proton beam writing (PBW). In the irradiated Agar material the polysaccharides are split into oligosaccharides which can easily be washed off leaving Agar-free areas for cell adhesion. The beam diameter of 1 μm allows the fabrication of compartments accommodating single cells which are connected by micrometer-sized channels. Using the external beam the production process is very fast. Up to 50 Petri dishes can be produced per day which makes this technique very suitable for biological investigations which require large throughputs.     

Enhancement of etch rate for preparation of nano-sized ion-track membranes of poly(vinylidene fluoride): Effect of pretreatment and high-LET beam irradiation

We investigated how pretreatment and high-LET beam irradiation affected the ion-track dissolution rate in poly(vinylidene fluoride) (PVDF) films by SEM observations and conductometric analysis in order to develop the preparation methodology of nano-sized ion-track membranes. PVDF thin films irradiated with four types of ion beams were exposed to a 9 mol/dm³ KOH aqueous solution after their storage in air at 120 °C. This heating treatment was found to enhance the etch rate in the latent track, both in the inner core and outer halo regions, without changing that in the bulk, probably due to the formation of parasitic oxidation products facilitating the introduction of the etching agent to improve the etchability. Additionally, the irradiation of heavier higher-LET ions, causing each track to more activated sites (like radicals), was preferable for achieving effective etching.     

Development of a high intensity Al beam from SiC targets for accelerated beam experiments at ISAC

An intense beam of ^26gAl has been developed for accelerated beam experiments at TRIUMF’s ISAC facility. Studies of the on-line production of Al radionuclides from thick silicon carbide targets have been performed as part of a program of beam development for astrophysical reaction studies at ISAC. While the release of short-lived Al nuclides from SiC was found to be slow, development of new target material forms and high-power target containers has allowed operation of SiC targets with proton currents of up to 70 μA on target. In addition, operation with the TRIUMF resonant ionization laser ion source (TRILIS) has produced ^26gAl beam intensities of 5.1 × 10¹⁰ s⁻¹.     

Ion-luminescence properties of GaN films being developed for IPEM

Radiation effects microscopy (REM) for the next generation integrated circuits (ICs) will require GeV ions both to provide high ionization and to penetrate the thick overlayers in present day ICs. These ion beams can be provided by only a few cyclotrons in the world. Since it is extremely hard to focus these higher-energy ions, we have proposed the ion photon emission microscope (IPEM) that allows the determination of the ion hits by focusing the emitted photons to a position sensitive detector. The IPEM needs a thin luminescent foil that has high brightness, good spatial resolution and does not change the incident ion’s energy and direction significantly. Available organic-phosphor foils require a large thickness to produce enough photons, which results in poor spatial resolution. To solve this problem, we have developed thin, lightly doped n-type GaN films that are extremely bright. We have grown high quality GaN films on sapphire using metal organic chemical vapor deposition (MOCVD), detached the films from the substrate using laser ablation, and made them self-supporting. The smallest foils have 1 mm² area and 1 μm thickness. The optical properties, such as light yield, spectrum and decay times were measured and compared to those of conventional phosphors, by using both alpha particles from a radioactive source and 250 keV ions from an implanter. We found that the GaN performance strongly depends on composition and doping levels. The conclusion is that 1-2 μm GaN film of a 1 mm² area may become an ideal ion position detector.     

Adhesion of proton beam written high aspect ratio hydrogen silsesquioxane (HSQ) nanostructures on different metallic substrates

Hydrogen silsesquioxane (HSQ) behaves as a negative resist under MeV proton beam exposure. HSQ is a high-resolution resist suitable for production of tall (<1.5 μm) high aspect ratio nanostructures with dimensions down to 22 nm. High aspect ratio HSQ structures can be used in many applications, e.g. nanofluidics, biomedical research, etc. Isolated HSQ nanostructures, however, tend to detach from substrates during the development process due to the weak adhesive forces between the resist and the substrate material. Larger proton fluences were observed to promote the adhesion. To determine an optimal substrate material and the proton irradiation doses for HSQ structures, a series of 2 μm long and 60-600 nm wide free-standing lines were written with varying fluences of 2 MeV protons in 1.2 μm thick HSQ resist spun on Ti/Si, Cr/Si and Au/Cr/Si substrates. The results indicate that the Ti/Si substrate is superior in terms of adhesion, while Au/Si is the worst. Cr/Si is not suitable as a substrate for HSQ resist because debris was formed around the structures, presumably due to a chemical reaction between the resist and Cr.     

Correlation between ion beam parameters and physical characteristics of nanostructures fabricated by focused ion beam

We report a study of the physical characteristics of the pillars of C, Pt and W grown by 10-30 keV Ga focused ion beam (FIB) as a function of Ga ion flux, and present a quantitative analysis of the elements using energy-dispersive analysis of X-rays (EDAX). All the FIB grown pillars exhibit a rough morphology with whisker like protrusions on the cylindrical surface and broadening of the base as compared to the nominal size. For a constant fluence, the height of the pillar initially increases and then reduces after going through a maximum as a function of ion flux in all the cases. The compositional analysis shows good metallic quality for Pt structures but reveals significant contamination of Ga in C and Ga and C in W structures at higher ion fluxes. Explanation to all these observations has been sought in the light of secondary ion and electron effects and the different processes involved which lead to the FIB induced deposition.     

MeV-ion beam analysis of the interface between filtered cathodic arc-deposited a-carbon and single crystalline silicon

Amorphous carbon (a-C) films were deposited on Si(1 0 0) wafers by a filtered cathodic vacuum arc (FCVA) plasma source. A negative electrical bias was applied to the silicon substrate in order to control the incident energy of carbon ions. Effects of the electrical bias on the a-C/Si interface characteristics were investigated by using standard Rutherford backscattering spectrometry (RBS) in the channeling mode with 2.1-MeV He²⁺ ions. The shape of the Si surface peaks of the RBS/channeling spectra reflects the degree of interface disorder due to atomic displacement from the bulk position of the Si crystal. Details of the analysis method developed are described. It was found that the width of the a-C/Si interface increases linearly with the substrate bias voltage but not the thickness of the a-C film.     

Release of Al from SiC targets used for radioactive ion beam production

On-line targets of silicon carbide have been used to produce radioactive ion beams (RIB) at TRIUMF’s ISAC facility. Surface ionized beams of Li, Na and Al from SiC targets have been delivered to a variety of experiments. While yields of Li and Na radionuclide beams have been high enough to meet experimental requirements, the yields of radio-aluminums have been very low in comparison to in-target production estimates. The properties of SiC relevant to radioactive Al ion beam production are reviewed and on-line measurements of radiogenic Li, Na and Al from SiC are presented. Diffusion, effusion and formation of stable phases are found to strongly affect the release of radio-aluminum from SiC, greatly reducing overall Al RIB production efficiency. In comparison, the production of radio-sodium beams from SiC is found to be relatively efficient.     

Thickness and MeV Si ions bombardment effects on the thermoelectric properties of Ce3Sb10 thin films

The three single layer Ce₃Sb₁₀ thin films were grown on silicon dioxide and quartz (suprasil) substrates with thicknesses of 297, 269 and 70 nm using ion beam assisted deposition (IBAD) technique. The high-energy cross plane Si ion bombardments with constant energy of 5 MeV have been performed with varying fluence from 1 × 10¹², 1 × 10¹³, 1 × 10¹⁴, 1 × 10¹⁵ ions/cm². The Si ions bombardment modified the thermoelectric properties of films as expected. The fluence and temperature dependence of cross plane thermoelectric parameters that are Seebeck coefficient, electrical and thermal conductivities were determined to evaluate the dimensionless figure of merit, ZT. Rutherford backscattering spectrometry (RBS) enabled us to determine the elemental composition of the deposited materials and layer thickness of each film.     

Complementary use of ion beam elastic backscattering and recoil detection analysis for the precise determination of the composition of thin films made of light elements

Rutherford backscattering spectrometry (RBS) is a well known powerful technique to obtain depth profiles of the constituent elements in a thin film deposited on a substrate made of lighter elements. In its standard use the probing beam is typically 2 MeV He. Its capabilities to obtain precise composition profiles are severely diminished when the overlaying film is made of elements lighter than the substrate. In this situation the analysis of the energy of the recoiled element from the sample in the elastic scattering event, the ERDA technique may be advantageous. For the detection of light elements it is also possible to use beams at specific energies producing elastic resonances with these light elements to be analyzed, with a much higher scattering cross sections than the Rutherford values. This technique may be called non-RBS. In this work we report on the complementary use of ERDA with a 30 MeV Cl beam and non-RBS with 1756 keV H ions to characterize thin films made of boron, carbon and nitrogen (BCN) deposited on Si substrates.     

Proton beam writing of long, arbitrary structures for micro/nano photonics and fluidics applications

The last decade has seen proton beam writing maturing into a versatile lithographic technique able to produce sub-100 nm, high aspect ratio structures with smooth side walls. However, many applications in the fields of photonics and fluidics require the fabrication of structures with high spatial resolution that extends over several centimetres. This cannot be achieved by purely magnetic or electrostatic beam scanning due to the large off-axis beam aberrations in high demagnification systems. As a result, this has limited us to producing long straight structures using a combination of beam and stage scanning. In this work we have: (1) developed an algorithm to include any arbitrary pattern into the writing process by using a more versatile combination of beam and stage scanning while (2) incorporating the use of the ubiquitous AutoCAD DXF (drawing exchange format) into the design process. We demonstrate the capability of this approach in fabricating structures such as Y-splitters, Mach-Zehnder modulators and microfluidic channels that are over several centimetres in length, in polymer. We also present optimisation of such parameters as scanning speed and scanning loops to improve on the surface roughness of the structures. This work opens up new possibilities of using CAD software in PBW for microphotonics and fluidics device fabrication.     

Method based on isotope ratio mass spectrometry for evaluation of carbon activation in the reactor graphite

The general idea of this work is to introduce an evaluation method to restore the irradiation parameters of graphite or other carbonaceous materials using experimental and modelling results of ¹³C generation in the irradiated material. The method is based on coupling of stable isotope ratio mass spectrometry and computer modelling of the reactor core to evaluate the realistic characteristics of the reactor core such as the neutron fluence in any position of the reactor graphite stack or other graphite constructions.The generation of carbon isotopes ¹³C and ¹⁴C in the irradiated graphite of the RBMK-1500 reactor has been estimated by modelling of the reactor core with computer codes MCNPX and CINDER90. Good agreement of simulated and measured Δ¹³C/¹²C values in graphite of the central part of the reactor core indicates that the neutron flux (1.40 × 10¹⁴ n/cm² s) is modelled accurately in the graphite sleeve of the fuel channel. The simulated activity of ¹⁴C is compared with the one measured by the β spectrometry technique. Results indicate that production of ¹⁴C from ¹⁴N in the RBMK-1500 reactor is considerable and has to be taken into account in order to make proper evaluation of ¹⁴C activity. Measured ¹⁴C specific activity values correspond to 15 ± 4 ppm impurity of ¹⁴N in graphite samples from the RBMK-1500 reactor core.     

Analysis of the potential for sub-eV Ps beams

Understanding the interactions of Ps at low energies has challenged researchers due to the inability to create Ps near thermal energies in a directed fashion. As a result, previous attempts to understand interactions such as the scattering cross-section (σ) between Ps and other atoms have relied on indirect methods. Examples are the measurements of the thermalization rate of Ps in a gas environment or lifetime measurements in various systems. In analyzing the pore size of certain nanotube materials we have observed 3-10% of incident positrons form long lived Ps within the sample. Due to the alignment of these tubes we expect Ps emitted from them to be highly directional. By focusing a time-tagged positron beam on these samples we will use the resulting directional Ps emitted at near thermal energies for various scattering experiments.     

Fabrication of uniform ZrC coating layer for the coated fuel particle of the very high temperature reactor

Fuel for the very high temperature reactor is required to be used under severer irradiation conditions and higher operational reactor temperatures than those of present high temperature gas cooled reactors. Japan Atomic Energy Agency has developed zirconium carbide (ZrC)-coated fuel particles previously in laboratory scale which are expected to maintain their integrity at higher temperatures and burnup conditions than conventional silicon carbide-coated fuel particles. As one of the important R&D items, ZrC coating process development has been started in the year 2004 to determine the coating conditions to fabricate uniform structure of ZrC layers by using a new large-scale coater up to 0.2 kg batch. It was thought that excess carbon formed in the ZrC layer under the oscillation of coating temperature would cause non-uniformity of the ZrC layer. Finally, uniform ZrC coating layer has been fabricated successfully by adjusting the time constant of the coater and keeping the coating temperature at around 1400 °C.     

PIXE and PIGE techniques for the analysis of Antarctic ice dust and continental sediments

An analytical procedure has been implemented in this work for an accurate geochemical characterization and quantitative analysis of the fine dust (particles diameter < 5 μm) trapped in Antarctic ice cores and the fine fraction of potential source areas (PSA) sediments by size selection, filtering and PIXE-PIGE combined measurements. The underestimation of concentrations of the lighter elements, like Na, Mg, Al and Si, due to X-ray self-absorption inside each individual aerosol particle, was also evaluated and the analytical overall accuracy tested by means of measurements performed on size selected certified mineral standards.     

Convolution approximation for the energy loss, ionization probability and straggling of fast ions

In this work we describe an extension of the convolution approximation for the ionization probability and energy-loss straggling as a function of the impact parameter for swift ions. Analytical formulas for these quantities are derived and compared to full first-order Born calculations. The physical inputs of the model are the electron density and oscillators strengths of the target as well as the screening function of the projectile (in the case of dressed ions). A very good agreement is obtained for all impact parameters. In addition, we propose a general schema to add contributions from distant and close collisions. In this way physical processes arising from large and small impact parameters can be easily included into a single expression valid for all impact parameters. This model is then used to investigate the projectile-charge q dependence of ionization, stopping and straggling cross-sections.     

A method for the quantification of total xenon concentration in irradiated nuclear fuel with SIMS and EPMA

A new method for the quantitative determination of the total xenon concentration in irradiated nuclear fuel is presented. The SIMS measurement of xenon enables the detection of the gas filling bubbles which are not detected with EPMA. The quantification is achieved using the EPMA data as reference at position where no or nearly no bubbles are detected. A new approach using the complementary information given by EPMA, SEM and SIMS is proposed, it opens new horizons for the characterisation of fission gases in irradiated nuclear fuel.     

Dynamic dependence of the interaction potentials for grazing scattering of fast atoms from metal and insulator surfaces

For scattering of fast atoms from metal and insulator surfaces under axial channeling conditions pronounced peaks in the angular distributions of scattered projectiles are interpreted in terms of rainbow scattering. The angular position of such “rainbow peaks” are closely related to the interaction potential and its corrugation in the topmost surface region. We have scattered N and O atoms, with energies ranging from 10 to 70 keV, from clean and flat Al(0 0 1) and LiF(0 0 1) surfaces along low index axial directions in the surface plane and studied the positions of the rainbow peaks as function of the kinetic energy of the atomic projectiles normal to the surface. For the insulator surface the rainbow angle does not depend on projectile energy for constant normal energy, whereas for the metal surface we find pronounced dynamic effects. We interpret this different behaviour as arising from a projectile energy dependent contribution to the underlying interaction potentials owing to embedding the projectiles into the free electron gas in the selvedge of the surfaces, which is present for the metals but absent for insulators.     

Technique for measuring angular correlations and g-factors of excited states with large multi-detector arrays: An application to neutron rich nuclei produced by the spontaneous fission of Cf

Triple coincidences between prompt γ-rays emitted in the spontaneous fission of ²⁵²Cf were measured with Gammasphere. These data are used to measure the angular correlation of cascades of γ-rays from excited states of neutron rich fission fragments stopped in an unmagnetized iron foil. The hyperfine fields in the iron lattice cause attenuations of the angular correlations between γ-rays emitted from the excited states which have sufficiently long lifetimes. This attenuation is measured and used to calculate the g-factors of excited states in many neutron rich nuclei.